He was associated with Washington University for 68 years, serving as assistant, associate, and full professor of geology, chair of the department, dean of the Graduate School of Arts and Sciences, vice chancellor–dean of faculties, and chancellor. During his one-year stewardship as chancellor before mandatory retirement, he steered the course through a time of transition and along the way reduced the university's debt from $1.5 million to $30,000.

He died in St. Louis in 1995 at age 97. Washington University Chancellor William H. Danforth said at the time of Tolman's death, "Carl Tolman was for 68 years one of the great people at Washington University. As a friend, as a faculty member, and as an academic leader, he was always farsighted and wise and kind and gentle."